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Multiscale Design of Aerosol Synthesis of Nanomaterials

Applicant Pratsinis Sotiris E.
Number 149144
Funding scheme Project funding (Div. I-III)
Research institution Institut für Verfahrenstechnik ETH Zürich
Institution of higher education ETH Zurich - ETHZ
Main discipline Mechanical Engineering
Start/End 01.10.2013 - 30.09.2016
Approved amount 359'643.00
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All Disciplines (2)

Discipline
Mechanical Engineering
Other disciplines of Engineering Sciences

Keywords (4)

Molecular Dynamics; Sintering; Nanostructured Materials; Flame Aerosol Reactors

Lay Summary (German)

Lead
Nanomaterialeigenschaften verstehen wir heutzutage besser und so konnten funktionelle Materialien entwickelt werden. Wenig bekannt ist aber, ob diese Eigenschaften auch bei der Grossproduktion erhalten bleiben. Die Verknüpfung von mehreren Modellen, welche verschiedene Längen- und Zeit-Grössenordnungen sowie die Teilchendynamik mit der Strömungsmechanik eines Prozesses kombinieren, ermöglicht eine vereinfachte Auslegung der Verfahrenstechnik und erlaubt die Synthese neuer Materialien.
Lay summary

Das Ziel dieses Projekt ist die Dynamik von Gasphasenpartikel-Reaktoren und die Partikelbildung in verschieden Längen- und Zeit-Grössenordnungen zu beschreiben indem Kontinuums-, Mesoskala-, molekulardynamische und auch quantenmechanische Modelle zusammen geführt werden. Durch die systematische Forschung wird ein fundiertes Verständnis geschaffen für die Kontrollmöglichkeiten der Partikelbildung, durch Koagulation und Verschmelzung, und der Produkteigenschaften, wie unter anderem Partikelgrösse, -morphology und –kristallinität. Die Koagulation von Nanopartikeln, welche eine sich schnell ändernde Struktur haben, kann zum Beispiel zu a) harten Agglomeraten führen, welche in den Bereichen wie Katalyse und Elektronik begehrt sind, oder zu b) weichen Agglomeraten, welche für Nanoverbundwerkstoffe und flüssigen Suspensionen viel versprechend sind. Ein solcher Prozess kann quantitativ durch Kontinuumsmodelle verfolgt werden, mit Hilfe von mesoskaligen Simulationen  welche die Restrukturierung von Agglomeraten/Aggregaten mit Molekular dynamischen Modellen berechnet. Diese Simulationen werden systematisch mit Aerosol-(Trägheit) und Material-(Röntgenbeugung bei kleinen Winkeln, Stickstoff-Adsorption)  Messungen verglichen, diese Messgeräte sind in unseren wie auch anderen Laboratorien vorhanden. Der Fokus liegt dabei aber immer auf der jeweiligen Anwendung (z.B. Photokatalyse). Diese Forschung trägt zum Grundlagenwissen bei und will Prozessparameter mit den Nanopartikeleigenschaften verbinden, ausgehend von fundamentalen Grundgleichungen. Dadurch wird die Herstellung von Nanomaterialien auf eine wissenschaftlich, standfeste Basis gestellt. Ein Schwerpunkt ist auf die systematische Kontrolle der Struktur von Nanomaterialen gelegt. Im Speziellen soll das Verständnis der Dynamik von Agglomeraten und Aggregaten im frei molekularen wie auch im kontinuierlichen Wachstumsbereich gefördert werden.

Direct link to Lay Summary Last update: 27.09.2013

Responsible applicant and co-applicants

Employees

Publications

Publication
Single Pd atoms on TiO 2 dominate photocatalytic NO x removal
Fujiwara Kakeru, Pratsinis Sotiris E. (2018), Single Pd atoms on TiO 2 dominate photocatalytic NO x removal, in Applied Catalysis B: Environmental, 226, 127-134.
Mobility and settling rate of agglomerates of polydisperse nanoparticles
Spyrogianni Anastasia, Karadima Katerina S., Goudeli Eirini, Mavrantzas Vlasis G., Pratsinis Sotiris E. (2018), Mobility and settling rate of agglomerates of polydisperse nanoparticles, in The Journal of Chemical Physics, 148(6), 064703-064703.
Surface Composition and Crystallinity of Coalescing Silver–Gold Nanoparticles
Goudeli Eirini, Pratsinis Sotiris E. (2017), Surface Composition and Crystallinity of Coalescing Silver–Gold Nanoparticles, in ACS Nano, 11(11), 11653-11660.
Flame synthesis of functional materials and devices: Surface growth and aggregation
Kelesidis G. Goudeli E. and Pratsinis S.E. (2016), Flame synthesis of functional materials and devices: Surface growth and aggregation, in Proceedings of the Combustion Institute, 36(1), 29-50.
Atomically dispersed Pd on nanostructured TiO2 for NO removal by solar light
Fujiwara K. Pratsinis S. E. (2016), Atomically dispersed Pd on nanostructured TiO2 for NO removal by solar light, in AIChE J., 63(1), 139-146.
Coagulation of Agglomerates Consisting of Polydisperse Primary Particles
Goudeli E. Eggersdorfer M.L. and Pratsinis S.E. (2016), Coagulation of Agglomerates Consisting of Polydisperse Primary Particles, in Langmuir, 32(36), 9276-9285.
Agglomeration with polydisperse primary particles in the free molecular regime
Goudeli E. Eggersdorfer M.L. and Pratsinis S.E. (2016), Agglomeration with polydisperse primary particles in the free molecular regime, in Langmuir, 32, 9276-9285.
Crystallinity dynamics of gold nanoparticles during sintering or coalescence
Goudeli E. and Pratsinis S.E. (2016), Crystallinity dynamics of gold nanoparticles during sintering or coalescence, in AIChE J. , 62, 589-598.
Gas-phase manufacturing of nanoparticles: Molecular Dynamics and Mesoscale Simulations
Goudeli E. and Pratsinis S.E. (2016), Gas-phase manufacturing of nanoparticles: Molecular Dynamics and Mesoscale Simulations, in Particul. Sci. Technol. , 34, 483-493.
Pd subnano-clusters on TiO2 for solar-light removal of NO
Fujiwara K. Müller U. Pratsinis S.E. (2016), Pd subnano-clusters on TiO2 for solar-light removal of NO, in ACS catalysis, 6, 1887-1893.
Sampling and dilution of nanoparticles at high temperature
Goudeli E. Gröhn A.J. and Pratsinis S.E. (2016), Sampling and dilution of nanoparticles at high temperature, in Aerosol Sci. Technol. , 50, 591-604.
Aggregate characteristics accounting for the evolving fractal-like structure during coagulation and sintering
Goudeli E. Eggersdorfer M.L. and Pratsinis S.E. (2015), Aggregate characteristics accounting for the evolving fractal-like structure during coagulation and sintering, in J. Aerosol Sci. , 89, 58-68.
Coagulation – agglomeration of fractal-like particles: structure and self-preserving size distribution
Goudeli E. Eggersdorfer M.L. and Pratsinis S.E. (2015), Coagulation – agglomeration of fractal-like particles: structure and self-preserving size distribution, in Langmuir , 31, 1320-1327.
Enhanced Ag+ ion release from aqueous nanosilver suspensions by absorption of ambient CO2
Fujiwara K. Sotiriou G.A. Pratsinis S.E. (2015), Enhanced Ag+ ion release from aqueous nanosilver suspensions by absorption of ambient CO2, in Langmuir, 31, 5284-5290.
Visible-light active black TiO2-Ag/TiOx particles
Fujiwara K. Deligiannakis Y. Skoutelis C.G. Pratsinis S.E. (2014), Visible-light active black TiO2-Ag/TiOx particles, in Appl. Catal. B-Environ. , 154-155, 9-15.

Collaboration

Group / person Country
Types of collaboration
University of Patras, Prof. Vlasios Mavrantzas Greece (Europe)
- Publication
EMPA, Ulrich Müller Switzerland (Europe)
- Publication
University of Ioannina, Prof. Yiannis Deligiannakis Greece (Europe)
- Publication
University of Patras, Katerina Karadima Greece (Europe)
- Publication
Novartis, Dr. Maximilian Eggersdorfer Switzerland (Europe)
- Publication
Karolinska Institutet, Prof. Georgios Sotiriou Sweden (Europe)
- Publication
University of Colorado Boulder, Dr. Arto Gröhn United States of America (North America)
- Publication

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
European Aerosol Conference Poster Surface composition during sintering of silver-gold alloyed nanoparticles 04.09.2016 Tours, France Pratsinis Sotiris E.; Goudeli Eirini;
European Aerosol Conference Talk given at a conference Palladium subnano-clusters on titania for solar photocatalytic NO removal. 04.09.2016 Tours, France Pratsinis Sotiris E.; Fujiwara Kakeru;
European Aerosol Conference Talk given at a conference The crystal structure and sintering of coalescing gold nanoparticles and its alloys 04.09.2016 Tours, France Goudeli Eirini; Pratsinis Sotiris E.;
European Aerosol Conference Poster Agglomeration of polydisperse primary particle in the free molecular regime 04.09.2016 Tours, France Eggersdorfer Maximilian; Pratsinis Sotiris E.; Goudeli Eirini;
European Aerosol Conference Poster One-step synthesis of atomically dispersed palladium on titania for NO removal 04.09.2016 Tours, France Pratsinis Sotiris E.; Fujiwara Kakeru;
International Symposium on Combustion Poster Atomically dispersed noble metals on titania by one-step flame spray pyrolysis 31.07.2016 Seoul, Korean Republic (South Korea) Pratsinis Sotiris E.; Fujiwara Kakeru;
International Conference on Photochemical Conversion and Storage of Solar Energy Poster Atomically dispersed Pd on TiO2 by one-step flame spray pyrolysis 25.07.2016 St. Petersburg, Russia Pratsinis Sotiris E.; Fujiwara Kakeru;
International Conference on Photochemical Conversion and Storage of Solar Energy Talk given at a conference Solar photocatalytic NO removal by subnanoclustered Pd on TiO2 25.07.2016 St. Petersburg, Russia Fujiwara Kakeru; Pratsinis Sotiris E.;
20th ETH Conference on Combustion Generated Nanoparticles Poster Agglomeration with polydisperse primary particles in the free molecular regime 13.06.2016 Zurich, Switzerland Pratsinis Sotiris E.; Eggersdorfer Maximilian; Goudeli Eirini;
Materials and Processing Graduate Symposium Poster Sintering rate and crystal structure of gold nanoparticles by molecular dynamics 09.06.2016 Zurich, Switzerland Goudeli Eirini; Pratsinis Sotiris E.;
PARTEC International Congress on Particle Technology Poster Sintering rate and crystal structure of gold nanoparticles by molecular dynamics 19.04.2016 Nuremberg, Germany Pratsinis Sotiris E.; Goudeli Eirini;
PARTEC Talk given at a conference Highly active Pd/TiO2 photocatalyst under solar light 19.04.2016 Nuremberg, Germany Pratsinis Sotiris E.; Fujiwara Kakeru;
PARTEC International Congress on Particle Technology Poster Coagulation – agglomeration of fractal-like particles 19.04.2016 Nuremberg, Germany Pratsinis Sotiris E.; Goudeli Eirini;
PARTEC International Congress on Particle Technology Poster The effect of sampler design on nanoparticle sizing 19.04.2016 Nuremberg, Germany Goudeli Eirini; Pratsinis Sotiris E.;
PARTEC International Congress on Particle Technology Talk given at a conference Agglomeration with polydisperse primary particles in the free molecular regime 19.04.2016 Nuremberg, Germany Goudeli Eirini; Pratsinis Sotiris E.; Eggersdorfer Maximilian;
European Aerosol Conference Poster The effect of primary particle polydispersity in the evolving agglomerate structure and size distribution 09.04.2016 Tours, France Eggersdorfer Maximilian; Goudeli Eirini; Pratsinis Sotiris E.;
MRS Fall Meeting Poster Enhanced Ag+ ion release from aqueous nanosilver suspensions by absorption of ambient CO2 29.11.2015 Boston, United States of America Fujiwara Kakeru; Pratsinis Sotiris E.;
AIChE Annual Meeting Talk given at a conference The crystal structure of coalescing Au and its alloy nanoparticles by molecular dynamics 08.11.2015 Salt Lake City, UT, United States of America Pratsinis Sotiris E.; Goudeli Eirini;
AIChE Annual Meeting Poster Sintering rate and crystallinity dynamics of gold nanoparticles by atomistic simulations 08.11.2015 Salt Lake City, United States of America Goudeli Eirini; Pratsinis Sotiris E.;
AIChE Annual Meeting Talk given at a conference The effect of sampler design on nanoparticle sizing 08.11.2015 Salt Lake City, United States of America Goudeli Eirini; Pratsinis Sotiris E.;
AIChE Annual Meeting Poster Multiscale design of gas-phase synthesis of nanomaterials 08.11.2015 Salt Lake City, United States of America Goudeli Eirini; Pratsinis Sotiris E.;
AAAR Annual Meeting Poster The effect of sampler design of nanoparticle sizing 12.10.2015 Minneapolis, United States of America Goudeli Eirini; Pratsinis Sotiris E.;
Asian Particle Technology Symposium Poster Enhanced Ag+ ion release from aqueous nanosilver suspensions by absorption of ambient CO2 15.09.2015 Seoul, Korean Republic (South Korea) Pratsinis Sotiris E.; Fujiwara Kakeru;
Asian Particle Technology Symposium Talk given at a conference Solar-light active TiOx photocatalyst by flame spray pyrolysis 15.09.2015 Seoul, Korean Republic (South Korea) Fujiwara Kakeru; Pratsinis Sotiris E.;
SCEJ fall meeting Poster Crystallization of TiOx (x < 2) by flame spray pyrolysis and post-annealing 09.09.2015 Hokkaido, Japan Pratsinis Sotiris E.; Fujiwara Kakeru;
European Aerosol Conference Poster Crystallinity Dynamics during Coalescence of Gold Nanoparticles 06.09.2015 Milan, Italy Goudeli Eirini; Pratsinis Sotiris E.;
European Aerosol Conference Talk given at a conference The effect of sampler design on nanoparticle sizing at high temperatures 06.09.2015 Milan, Italy Goudeli Eirini; Pratsinis Sotiris E.;
19th ETH Conference on Combustion Generated Nanoparticles Poster Coagulation-agglomeration of fractal-like particles 28.06.2015 Zurich, Switzerland Pratsinis Sotiris E.; Goudeli Eirini; Eggersdorfer Maximilian;
19th ETH Conference on Combustion Generated Nanoparticles, ETH Zürich, Switzerland Poster The effect of sampler design of nanoparticles sizing at high temperatures 28.06.2015 Zurich, Switzerland Goudeli Eirini; Pratsinis Sotiris E.;
Materials and Processing Graduate Symposium Poster Aggregate characteristics accounting for the evolving fractal-like structure during coagulation and sintering 03.06.2015 Zurich, Switzerland Goudeli Eirini; Pratsinis Sotiris E.; Eggersdorfer Maximilian;
MRS Fall Meeting Poster Visible-light active black TiOx-Ag/TiO2 30.11.2014 Boston, United States of America Fujiwara Kakeru; Pratsinis Sotiris E.;
Fall Meeting on the Materials Research Society (MRS) Poster Sintering Rate and Crystal Structure of Gold Nanoparticles by Molecular Dynamics 30.11.2014 Boston, United States of America Goudeli Eirini; Pratsinis Sotiris E.;
Fall Meeting of the Materials Research Society (MRS) Talk given at a conference Coagulation – Agglomeration of Fractal-like Aerosols: Structure & Self-Preserving Size Distribution 30.11.2014 Boston, MA, United States of America Eggersdorfer Maximilian; Pratsinis Sotiris E.; Goudeli Eirini;
Fall Meeting on the Materials Research Society (MRS) Poster The Asymptotic Structure and Size Distribution of Fractal-like Aerosols made by Agglomeration 30.11.2014 Boston, United States of America Goudeli Eirini; Eggersdorfer Maximilian; Pratsinis Sotiris E.;
MRS Fall Meeting Talk given at a conference Solar-light photocatalyst: surface-oxidized crystalline TiOx on Ag/TiO2 30.11.2014 Boston, United States of America Fujiwara Kakeru; Pratsinis Sotiris E.;
AIChE Annual Meeting Talk given at a conference Agglomeration of Fractal-like Particles 16.11.2014 Minneapolis, MN, United States of America Goudeli Eirini; Eggersdorfer Maximilian; Pratsinis Sotiris E.;
International Aerosol Conference Talk given at a conference Coagulation of Fractal-like Aerosols in the Transition Regime 28.08.2014 Busan, Korean Republic (South Korea) Goudeli Eirini; Eggersdorfer Maximilian; Pratsinis Sotiris E.;
International Aerosol Conference Talk given at a conference The effect of evolving fractal-like structure on product primary and agglomerate size & morphology during coagulation and sintering 28.08.2014 Busan, Korean Republic (South Korea) Pratsinis Sotiris E.; Goudeli Eirini; Eggersdorfer Maximilian;
International Aerosol Conference Poster The effect of diluter configuration on characterization of flame-made particles 28.08.2014 Busan, Korean Republic (South Korea) Goudeli Eirini; Eggersdorfer Maximilian; Pratsinis Sotiris E.;
International Conference on Photochemical Conversion and Storage of Solar Energy Talk given at a conference Visible-light active black Ag/TiOx particles 27.07.2014 Berlin, Germany Pratsinis Sotiris E.; Fujiwara Kakeru;
International Conference on Photochemical Conversion and Storage of Solar Energy Talk given at a conference Solar-light photocatalyst: surface-oxidized crystalline TiOx on Ag/TiO2 27.07.2014 Berlin, Germany Pratsinis Sotiris E.; Fujiwara Kakeru;
18th ETH Conference on Combustion Generated Nanoparticles Talk given at a conference Coagulation of Fractal-like Aerosols in the Transition Regime 22.06.2014 Zurich, Switzerland Goudeli Eirini; Eggersdorfer Maximilian; Pratsinis Sotiris E.;
Materials and Processing Graduate Symposium Poster Coagulation of Fractal-like Aerosols in the Transition Regime 05.06.2014 Zurich, Switzerland Pratsinis Sotiris E.; Goudeli Eirini; Eggersdorfer Maximilian;
MRS Fall Meeting Poster Ag+ ion release from nanosilver in aqueous solutions: Effect of size, pH and O2 concentration 01.12.2013 Boston, United States of America Fujiwara Kakeru; Pratsinis Sotiris E.;
AAAR Annual Meeting Poster Accounting for the Variable Df during Coagulation and Sintering of Fractal-like Particles 04.10.2013 Portland, United States of America Goudeli Eirini; Pratsinis Sotiris E.; Eggersdorfer Maximilian;


Awards

Title Year
2018 Inaugural GAeF PhD award by the German Association for Aerosol Research (Gesellschaft für Aerosolforschung) 2018
ETH medal for outstanding PhD thesis, 2016 2016
AIChE Annual Meeting, November 8 – 13, 2015, in Salt Lake City, UT, USA where Eirini Goudeli received the 3rd Best Poster Award at Particle Technology Forum Poster Session 2015
Fall Meeting of Materials Research Society (MRS), Symposium HH on Flame and High-Temperature Synthesis of Functional Nanomaterials, December 1 – 4, 2014, in Boston, MA, USA where Eirini Goudeli received a Best Presentation Award 2014
European Aerosol Conference (EAC), September 1 – 6, 2013, in Prague, Czech Republic where Eirini Goudeli received a Best Poster Award on Aerosol Fundamentals 2013

Associated projects

Number Title Start Funding scheme
182668 Tailor-made Carbonaceous Nanoparticles by Multiscale Combustion Design 01.01.2019 Project funding (Div. I-III)
119946 Flame-made Nanostructured Materials: Aerosol Dynamics at High Particle Concentration 01.04.2008 Project funding (Div. I-III)

Abstract

Today there is a better understanding of nanomaterial properties capitalizing a) on basic research in various fields of science and b) on advances in instrumentation and synthetic processes. This has led to new materials with a number of functionalities and potential applications including catalysts, sensors, biomaterials and even nutritional supplements to name a few that our laboratory has contributed. At the same time, however, little is known on how well nanomaterial properties are reproduced during large-scale manufacture of nanomaterials. So their widespread use largely depends on the development of economic and safe routes for their synthesis. Such materials are made primarily by wet or dry phase (aerosol) processes. The latter have distinct advantages for scale-up given the nanostructured commodities (e.g. carbon black, fumed oxides) available at the ton-scale in the market today. The manufacture of these commodities have taught us that the dynamics of aerosol reactors and product nanoparticle characteristics span 10 and 15 orders of magnitude in length and time. So systematic process design requires models for different length and time scales. These models can be distinguished into continuum, mesoscale, molecular dynamics and quantum mechanics ones that are interconnected for multiscale process design. That way the relationship between product properties and process variables can be built on a firm scientific basis. For example, reactor design for nano-oxides relies typically on particle coagulation and coalescence at various temperatures and residence times. Textbook coagulation rates for spherical particles do not hold for agglomerates of the typical fractal-like nanostructured materials. So, coagulation of nanoparticles with a rapidly evolving structure may result in a) hard agglomerates that are attractive in catalysis and electronics or b) soft agglomerates that are attractive in nanocomposites and liquid suspensions. Such a process can be followed quantitatively by continuum models using mesoscale simulations that describe restructuring of agg(lomer/reg)ates with a nanoparticle coalescence rate from molecular dynamics. Such simulations will be compared systematically to aerosol and material measurements in our and other laboratories.A further focus of this project is the crystallization dynamics of aerosol-made nanoparticles. Control of crystallinity is not as well understood as that of the various nanomaterial sizes. In fact, crystallinity is controlled rather empirically in practice. For example, Al-doping is used to lock rutile formation in gas-phase manufacture of pigmentary titania (a 3-billion dollar world-wide business). After all, the performance of many nanomaterials is often related to their crystal structure. So molecular dynamics will be applied to understand grain boundary mobility, structure and sintering of nanomaterials from first principles and compare with pertinent experimental data. This may help to design crystal phase composition and size which can affect also nanomaterial morphology. This project will assist the education of PhD students specializing in nanoparticle processing and expose BSc/MSc students to fascinating engineering science impacting a number of applications. Results will be presented at international conferences and submitted to refereed journals.
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